考察了氮气预处理温度对硫代硫酸铵预硫化的Mo/Al2O3催化剂噻吩加氢脱硫(HDS)活性的影响. 采用X射线衍射、高分辨电镜、光电子能谱、热重质谱和硫分析等方法对催化剂进行了表征. 结果表明,预硫化催化剂经80 ℃低温处理并于200 ℃氢气原位活化后噻吩转化率达到最高. 对于氮气低温预处理或常温干燥的预硫化催化剂,载体氧化铝被硫酸根修饰,减少了Mo与载体的相互作用,使得催化剂活化后硫化程度高, MoS2活性相呈多层的Ⅱ型结构,因而HDS活性高. 高于200 ℃的氮气热处理造成硫代硫酸铵的分解,并有少量的多层MoS2活性相生成,但高温热处理造成硫的流失使得活性金属活化后硫化程度偏低,而且MoS2活性相呈现单层的Ⅰ型结构,因而HDS活性较低.
参考文献
| [1] | Topsoe H;Clausen B S;Massoth F E;Anderson J R,Boudart M.Hydrotreating Catalysis:Science and Technology[M].Beilin:Springer-Verlag,1996:38. |
| [2] | 丁伯强,王鉴,董群,刘忠恩.加氢催化剂预硫化技术进展[J].石化技术与应用,2005(01):56-60. |
| [3] | Welch J G;Poyner P;Skelly R F .[J].Oil & Gas Journal,1994,92(41):56. |
| [4] | Berrebi G .[P].US 4?530?917,1985. |
| [5] | Dufresne P;Legall B;Berrebi G .[P].US 5?397?756,1995. |
| [6] | 于守智;高晓冬;陈若雷 .[P].CN 1200081C,2005. |
| [7] | 李彦鹏,刘大鹏,刘晓,柴永明,刘晨光.器外预硫化型MoNiP/γ-Al2O3催化剂的二苯并噻吩加氢脱硫活性[J].催化学报,2006(07):624-630. |
| [8] | Yamada S;Qian W H;Ishihare A;Wang G Li L Kabe T .[J].Sekiyu Gakkaishi-Journal of the Japan Petroleum Institute,2001,44(04):217. |
| [9] | 李彦鹏,刘大鹏,柴永明,刘晨光.器外预硫化型MoNiP/γ-Al2O3催化剂的加氢脱硫性能研究[J].石油炼制与化工,2006(05):15-19. |
| [10] | Murff S R;Carliste E A;Dufresne P;Rabehasaina H .[J].Preprints-American Chemical Society,Division of Petroleum Chemistry,1993,38(01):81. |
| [11] | De Wind M;Heinerman J J L H;Lee S L;Plantenga F L Johnson C C Woodward D C .[J].Oil & Gas Journal,1992,90(08):49. |
| [12] | Blashka S;Bond G;Ward D .[J].Oil & Gas Journal,1998,96(01):36. |
| [13] | 高玉兰,方向晨,王刚,曹凤兰,李崇慧.器外预硫化加氢催化剂的工业放大[J].炼油技术与工程,2005(04):34-35. |
| [14] | 刘畅,祁兴国,马守波,孙树成,赵法军.加氢催化剂器外预硫化技术进展[J].化学工程师,2006(01):33-38. |
| [15] | Berrebi G;Le Gall B .[P].US 5?139?983,1992. |
| [16] | Roumieu R;Boitiaux J P .[P].US 5?153?163,1992. |
| [17] | De Jong J I;Eisenhuth L;Schoonhoven J W F M;Van Hengstum A J .[P].US 5?139?990,1992. |
| [18] | 葛晖,李学宽,王建国,秦张峰,吕占军,杨英.硫代硫酸铵预硫化的MoO3/Al2O3催化剂的活化和加氢脱硫活性[J].催化学报,2008(09):921-927. |
| [19] | Hui Ge;Xuekuan Li;Zhangfeng Qin .Highly active Mo/Al2O3 hydrodesulfurization catalyst presulfided with ammonium thiosulfate[J].Catalysis Communications,2008(15):2578-2582. |
| [20] | La Parola V;Deganello G;Venezia A M .[J].Applied Catalysis A:General,2004,260(02):237. |
| [21] | Parham T G;Merrill R P .[J].Journal of Catalysis,1984,85(02):295. |
| [22] | De Boer M;Van Dillen A J;Koningsberger D C;Geus J W .[J].Japanese Journal of Applied Physics,1993,32(z32-2):460. |
| [23] | Topsoe H;Hinnemann B;Norskov J K;Lauritsen J V Besenbacher F Hansen P L Hytoft G Egeberg R G Knudsen K G .[J].Catalysis Today,2005,107-108:12. |
| [24] | Kouzu M;Uchida K;Kuriki Y;Ikazaki F .Micro-crystalline molybdenum sulfide prepared by mechanical milling as an unsupported model catalyst for the hydrodesulfurization of diesel fuel[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2004(1/2):241-249. |
| [25] | Alonso G;Berhault G;Aguilar A;Collins V Ornelas C Fuentes S Chianelli R R .[J].Journal of Catalysis,2002,208(02):359. |
| [26] | Hensen E J M;De Beer V H J;Van Veen J A R;Van Santen R A .[J].Catalysis Letters,2002,84(1-2):59. |
| [27] | Hinnemann B;Norskov J K;Topsoe H .[J].Journal of Physical Chemistry B,2005,109(06):2245. |
| [28] | SHANG Hong-Yan;LIU Chen-Guang;ZHAO Rui-Yu;WU Ming-Bo;WEI Fei .XPS Characterization of Carbon Nanotube Supported CoMo Hydrodesulfurization Catalysts[J].Chinese Journal of Chemistry,2004(11):1250-1256. |
| [29] | Texier S;Berhault G;Perot G;Diehl F .[J].Applied Catalysis A:General,2005,293:105. |
| [30] | Alstrup I;Chorkendorff I;Candia R;Clausen B S Topsoe H .[J].Journal of Catalysis,1982,77(02):397. |
| [31] | Duan A J;Wan G F;Zhao Zh;Xu Ch M Zheng Y Y Zhang Y Dou T Bao X J Chung K .[J].Catalysis Today,2007,119(1-4):13. |
| [32] | Van der Aalst M J M;De Beer V H J .[J].Journal of Catalysis,1977,49(03):247. |
| [33] | Arnoldy P;van den Heijkant J A M;De Bok G D;Moulijn J A .[J].Journal of Catalysis,1985,92(01):35. |
| [34] | Vissers J P R;Scheffer B;De Beer V H J;Moulijn J A Prins R .[J].Journal of Catalysis,1987,105(02):277. |
| [35] | Payen E;Kasztelan S;Houssenbay S;Szymanski R Grimblot J .[J].Journal of Physical Chemistry,1989,93(17):6501. |
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